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Practical high-temperature superconductors must be textured to minimize the reduction of the critical current density J(gb) at misoriented grain boundaries. Partial substitution of Ca for Y in YBa(2)Cu(3)O(7-delta) has shown significant improvement in J(gb) but the mechanisms are still not well understood. Here we report atomic-scale, structural and analytical electron microscopy combined with transport measurements on 7 degrees [001]-tilt Y(0.7)Ca(0.3)Ba(2)Cu(3)O(7-delta) and YBa(2)Cu(3)O(7-delta) grain boundaries, where the dislocation cores are well separated. We show that the enhanced carrier density, higher J(gb) and weaker superconductivity depression at the Ca-doped boundary result from a strong, non-monotonic Ca segregation and structural rearrangements on a scale of approximately 1 nm near the dislocation cores. We propose a model of the formation of Ca(2+) solute atmospheres in the strain and electric fields of the grain boundary and show that Ca doping expands the dislocation cores yet enhances J(gb) by improving the screening and local hole concentration.

Electromagnetic, atomic structure and chemistry changes induced by Ca-doping of low-angle YBa2Cu3O7–δ grain boundaries